Batteries

11 pages, 2117 KiB

Open AccessFeature PaperEditor’s ChoiceReview

Recycling of Lithium-Ion Batteries via Electrochemical Recovery: A Mini-Review

by Lu Yu, Yaocai Bai and Ilias Belharouak

Batteries 2024, 10(10), 337; https://doi.org/10.3390/batteries10100337 - 24 Sep 2024

Cited by 8 | Viewed by 6812

With the rising demand for lithium-ion batteries (LIBs), it is crucial to develop recycling methods that minimize environmental impacts and ensure resource sustainability. The focus of this short review is on the electrochemical techniques used in LIB recycling, particularly electrochemical leaching and electrodeposition. [...] Read more.

With the rising demand for lithium-ion batteries (LIBs), it is crucial to develop recycling methods that minimize environmental impacts and ensure resource sustainability. The focus of this short review is on the electrochemical techniques used in LIB recycling, particularly electrochemical leaching and electrodeposition. Our summary covers the latest research, highlighting the principles, progress, and challenges tied to these methods. By examining the current state of electrochemical recovery, this review intends to provide guidance for future advancements and enhance LIB recycling efficiency. Full article

(This article belongs to the Special Issue Lithium-Ion Battery Recycling)

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17 pages, 4493 KiB

Open AccessEditor’s ChoiceArticle

Improving Lithium-Ion Battery Performance: Nano Al₂O₃ Coatings on High-Mass Loading LiFePO₄ Cathodes via Atomic Layer Deposition

by Pejman Salimi, Gloria Gottardi, William G. Morais, Ruben Bartali, Nadhira Laidani and Edoardo Gino Macchi

Batteries 2024, 10(9), 304; https://doi.org/10.3390/batteries10090304 - 28 Aug 2024

Cited by 7 | Viewed by 4400

Abstract

Lithium iron phosphate (LiFePO₄ or LFP) is a promising cathode material for lithium-ion batteries (LIBs), but side reactions between the electrolyte and the LFP electrode can degrade battery performance. This study introduces an innovative coating strategy, using atomic layer deposition (ALD) to [...] Read more.

Lithium iron phosphate (LiFePO₄ or LFP) is a promising cathode material for lithium-ion batteries (LIBs), but side reactions between the electrolyte and the LFP electrode can degrade battery performance. This study introduces an innovative coating strategy, using atomic layer deposition (ALD) to apply a thin (5 nm and 10 nm) Al₂O₃ layer onto high-mass loading LFP electrodes. Galvanostatic charge–discharge cycling and electrochemical impedance spectroscopy (EIS) were used to assess the electrochemical performance of coated and uncoated LFP electrodes. The results show that Al₂O₃ coatings enhance the cycling performance at room temperature (RT) and 40 °C by suppressing side reactions and stabilizing the cathode–electrolyte interface (CEI). The coated LFP retained 67% of its capacity after 100 cycles at 1C and RT, compared to 57% for the uncoated sample. Post-mortem analyses, including scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS), were conducted to investigate the mechanisms behind the improved performance. These analyses reveal that Al₂O₃ coatings are highly effective in reducing LFP electrode degradation during cycling, demonstrating the potential of ALD Al₂O₃ coatings to enhance the durability and performance of LFP electrodes in LIBs. Full article

(This article belongs to the Special Issue Processes and Advances in Electrode Materials for Lithium-Ion Batteries)

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15 pages, 4783 KiB

Open AccessEditor’s ChoiceArticle

Anion Intercalation/De-Intercalation Mechanism Enabling High Energy and Power Densities of Lithium-Ion Capacitors

by Yang Zhang, Junquan Lao and Ping Xiao

Batteries 2024, 10(9), 296; https://doi.org/10.3390/batteries10090296 - 23 Aug 2024

Cited by 1 | Viewed by 1946

Abstract

The growing demands for electrochemical energy storage systems is driving the exploration of novel devices, with lithium-ion capacitors (LICs) emerging as a promising strategy to achieve both high energy density and fast charge capability. However, the low capacitance of commercial activated carbon (AC) [...] Read more.

The growing demands for electrochemical energy storage systems is driving the exploration of novel devices, with lithium-ion capacitors (LICs) emerging as a promising strategy to achieve both high energy density and fast charge capability. However, the low capacitance of commercial activated carbon (AC) cathode based on anion absorption/desorption limits LIC applications. Herein, commercial graphite is proposed as the cathode to construct an innovative AC (−)//graphite (+) system. The graphite cathode functions as anion hosting, allowing reversible intercalation/de-intercalation of anions into/from its interlayers. The as-designed AC (−)//graphite (+) full cell achieves stable cycling with 90.6% capacity retention after 200 cycles at 0.1 A g⁻¹ and a prolonged lifespan with 87.5% capacity retention after 5000 cycles at 0.5 A g⁻¹ with the upper cut-off voltage of 5.0 V, yielding a high average Coulombic efficiency (CE) of 99.3%. Moreover, the full cell exhibits a high energy density (>200 Wh kg⁻¹) and power density of 7.7 kW kg⁻¹ (calculated based on active mass in both electrodes). These performances exceed most LICs based on anions absorption/desorption on the surface of AC cathodes. This work explores an effective electrode revolution with the assistance of anion intercalation/de-intercalation chemistry for developing novel LICs with high energy and power densities. Full article

(This article belongs to the Special Issue Advanced Studies on High-Performance Metal-Ion Capacitors: Technologies, Systems and Applications)

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18 pages, 18755 KiB

Open AccessEditor’s ChoiceArticle

Experimental Study on Thermal Runaway Characteristics of High-Nickel Ternary Lithium-Ion Batteries under Normal and Low Pressures

by Ye Jin, Di Meng, Chen-Xi Zhao, Jia-Ling Yu, Xue-Hui Wang and Jian Wang

Batteries 2024, 10(8), 287; https://doi.org/10.3390/batteries10080287 - 12 Aug 2024

Cited by 4 | Viewed by 2500

Abstract

High-nickel (Ni) ternary lithium-ion batteries (LIBs) are widely used in low-pressure environments such as in the aviation industry, but their attribute of high energy density poses significant fire hazards, especially under low pressure where thermal runaway behavior is complex, thus requiring relevant experiments. [...] Read more.

High-nickel (Ni) ternary lithium-ion batteries (LIBs) are widely used in low-pressure environments such as in the aviation industry, but their attribute of high energy density poses significant fire hazards, especially under low pressure where thermal runaway behavior is complex, thus requiring relevant experiments. This study investigates the thermal runaway characteristics of LiNi_0.8Mn_0.1Co_0.1O₂ (NCM811) 18650 LIBs at different states of charge (SOCs) (75%, 100%) under various ambient pressures (101 kPa, 80 kPa, 60 kPa, 40 kPa). The results show that, as the pressure is decreased from 101 kPa to 40 kPa, the onset time of thermal runaway is extended by 28.2 s for 75% SOC and by 40.8 s for 100% SOC; accordingly, the onset temperature of thermal runaway increases by 19.3 °C for 75% SOC and by 33.5 °C for 100% SOC; the maximum surface temperature decreases by 70.8 °C for 75% SOC and by 68.2 °C for 100% SOC. The cell mass loss and loss rate slightly decrease with reduced pressure. However, ambient pressure has little impact on the time and temperature of venting as well as the voltage drop time. SEM/EDS analysis verifies that electrolyte evaporates faster under low pressure. Furthermore, the oxygen concentration is lower under low pressure, which consequently leads to a delay in thermal runaway. This study contributes to understanding thermal runaway characteristics of high-Ni ternary LIBs and provides guidance for their safe application in low-pressure aviation environments. Full article

(This article belongs to the Special Issue Advances in Lithium-Ion Battery Safety and Fire)

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21 pages, 5171 KiB

Open AccessEditor’s ChoiceArticle

Sustainable Battery Lifecycle: Non-Destructive Separation of Batteries and Potential Second Life Applications

by Gernot Schlögl, Stefan Grollitsch, Christian Ellersdorfer, Florian Feist, Christoph Kirschner, Josef Ecker and Franz Haas

Batteries 2024, 10(8), 280; https://doi.org/10.3390/batteries10080280 - 5 Aug 2024

Cited by 4 | Viewed by 3413

Abstract

Large quantities of battery systems will be discarded from electric vehicles in the future. Non-destructive separation of used electric vehicle (EV) traction batteries enables a second life of battery components, extraction of high value secondary materials, and reduces the environmental footprint of recycling [...] Read more.

Large quantities of battery systems will be discarded from electric vehicles in the future. Non-destructive separation of used electric vehicle (EV) traction batteries enables a second life of battery components, extraction of high value secondary materials, and reduces the environmental footprint of recycling and separation processes. In this study, the key performance indicators (KPIs) for the second life application of spent EV batteries are identified. Three battery packs are analyzed in terms of the joining techniques used—and possible separation techniques—considering only direct recycling methods. The components that can be recovered from these batteries are evaluated against the KPIs. This study shows that all the batteries analyzed allow a second life in stationary and semi-stationary electrical storage systems and marine applications when used at the pack and module levels. Two packs can be reused in electric vehicles such as forklifts. However, the feasibility of re-use in micro-mobility and consumer electronics is very limited. This study shows that technically feasible separation methods are dictated and constrained by the joining techniques used. As welding and adhesive bonding pose challenges to separation processes, future efforts should prioritize ‘design for disassembly’ to ensure sustainable battery life cycle management. Full article

(This article belongs to the Special Issue Sustainable Materials and Recycling Processes for Battery Production)

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38 pages, 9849 KiB

Open AccessEditor’s ChoiceReview

Binders for Li-Ion Battery Technologies and Beyond: A Comprehensive Review

by Muskan Srivastava, Anil Kumar M. R. and Karim Zaghib

Batteries 2024, 10(8), 268; https://doi.org/10.3390/batteries10080268 - 26 Jul 2024

Cited by 16 | Viewed by 16647

Abstract

The effects of global warming highlight the urgent need for effective solutions to this problem. The electrification of society, which occurs through the widespread adoption of electric vehicles (EVs), is a critical strategy to combat climate change. Lithium-ion batteries (LIBs) are vital components [...] Read more.

The effects of global warming highlight the urgent need for effective solutions to this problem. The electrification of society, which occurs through the widespread adoption of electric vehicles (EVs), is a critical strategy to combat climate change. Lithium-ion batteries (LIBs) are vital components of the global energy-storage market for EVs, and sodium-ion batteries (SIBs) have gained renewed interest owing to their potential for rapid growth. Improved safety and stability have also put solid-state batteries (SSBs) on the chart of top batteries in the world. This review examines three critical battery technologies: LIBs, SIBs, and SSBs. Although research has historically concentrated on heavier battery components, such as electrodes, to achieve high gravimetric density, binders, which comprise less than 5% of the battery weight, have demonstrated great promise for meeting the increasing need for energy storage. This review thoroughly examines various binders, focusing on their solubilities in water and organic solvents. Understanding binder mechanisms is crucial for developing binders that maintain strong adhesion to electrodes, even during volume fluctuations caused by lithiation and delithiation. Therefore, we investigated the different mechanisms associated with binders. This review also discusses failure mechanisms and innovative design strategies to improve the performance of binders, such as composite, conductive, and self-healing binders. By investigating these fields, we hope to develop energy storage technologies that are more dependable and efficient while also helping to satisfy future energy needs. Full article

(This article belongs to the Section Battery Materials and Interfaces: Anode, Cathode, Separators and Electrolytes or Others)

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36 pages, 3484 KiB

Open AccessEditor’s ChoiceReview

Environmental Aspects and Recycling of Solid-State Batteries: A Comprehensive Review

by Abniel Machín, María C. Cotto, Francisco Díaz, José Duconge, Carmen Morant and Francisco Márquez

Batteries 2024, 10(7), 255; https://doi.org/10.3390/batteries10070255 - 17 Jul 2024

Cited by 15 | Viewed by 11014

Abstract

Solid-state batteries (SSBs) have emerged as a promising alternative to conventional lithium-ion batteries, with notable advantages in safety, energy density, and longevity, yet the environmental implications of their life cycle, from manufacturing to disposal, remain a critical concern. This review examines the environmental [...] Read more.

Solid-state batteries (SSBs) have emerged as a promising alternative to conventional lithium-ion batteries, with notable advantages in safety, energy density, and longevity, yet the environmental implications of their life cycle, from manufacturing to disposal, remain a critical concern. This review examines the environmental impacts associated with the production, use, and end-of-life management of SSBs, starting with the extraction and processing of raw materials, and highlights significant natural resource consumption, energy use, and emissions. A comparative analysis with traditional battery manufacturing underscores the environmental hazards of novel materials specific to SSBs. The review also assesses the operational environmental impact of SSBs by evaluating their energy efficiency and carbon footprint in comparison to conventional batteries, followed by an exploration of end-of-life challenges, including disposal risks, regulatory frameworks, and the shortcomings of existing waste management practices. A significant focus is placed on recycling and reuse strategies, reviewing current methodologies like mechanical, pyrometallurgical, and hydrometallurgical processes, along with emerging technologies that aim to overcome recycling barriers, while also analyzing the economic and technological challenges of these processes. Additionally, real-world case studies are presented, serving as benchmarks for best practices and highlighting lessons learned in the field. In conclusion, the paper identifies research gaps and future directions for reducing the environmental footprint of SSBs, underscoring the need for interdisciplinary collaboration to advance sustainable SSB technologies and contribute to balancing technological advancements with environmental stewardship, thereby supporting the transition to a more sustainable energy future. Full article

(This article belongs to the Section Battery Processing, Manufacturing and Recycling)

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14 pages, 4677 KiB

Open AccessEditor’s ChoiceArticle

Development of Printed Pouch Film and Flexible Battery

by Gyeongseok Oh, Snigdha Paramita Mantry, Jae Ho Sim, Hyeon Woo Cho, Mijin Won, Hwamok Park, Jiyoung Park, Juhwan Lee and Dong Soo Kim

Batteries 2024, 10(7), 244; https://doi.org/10.3390/batteries10070244 - 8 Jul 2024

Viewed by 2368

Abstract

This study investigates the properties of various adhesives and assesses the effects of the coating and drying conditions of aluminum surface treatment agents on adhesion strength and chemical resistance. The adhesion between aluminum and the polymer film is improved through the application of [...] Read more.

This study investigates the properties of various adhesives and assesses the effects of the coating and drying conditions of aluminum surface treatment agents on adhesion strength and chemical resistance. The adhesion between aluminum and the polymer film is improved through the application of a surface treatment agent to the aluminum surface. This study examines the initial adhesive strength of a manufactured pouch film with respect to the drying temperature and time and evaluates its adhesive strength in the presence of moisture. The results indicate that the residual moisture on the aluminum surface weakens the adhesive strength and significantly affects electrolyte resistance. A noticeable reduction in strength was observed after water spraying, when the drying temperature and time were relatively low during the initial strength measurement. Among the adhesives used for aluminum and CPP lamination, olefin adhesives exhibit less susceptibility to electrolyte effects and have higher adhesive strengths compared to urethane and ester adhesives. Leveraging these characteristics, flexible pouch cells were manufactured and their stability was evaluated. The results confirm that the flexible cells demonstrate excellent stability, exhibiting potential for application in wearable devices. Full article

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16 pages, 3731 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Experimental Investigation on Thermal Runaway of Lithium-Ion Batteries under Low Pressure and Low Temperature

by Di Meng, Jingwen Weng and Jian Wang

Batteries 2024, 10(7), 243; https://doi.org/10.3390/batteries10070243 - 6 Jul 2024

Cited by 9 | Viewed by 3978

Abstract

Understanding the thermal runaway mechanism of lithium-ion batteries under low pressure and low temperature is paramount for their application and transportation in the aviation industry. This work investigated the coupling effects of ambient pressure (100 kPa, 70 kPa, 40 kPa) and ambient temperature [...] Read more.

Understanding the thermal runaway mechanism of lithium-ion batteries under low pressure and low temperature is paramount for their application and transportation in the aviation industry. This work investigated the coupling effects of ambient pressure (100 kPa, 70 kPa, 40 kPa) and ambient temperature (−15 °C, 0 °C, 25 °C) on thermal behaviors in an altitude temperature chamber. The experimental results indicate that lowering ambient pressure and temperature could attenuate the thermal runaway intensity, which is mainly attributable to the reduction in oxygen concentration and the increase in heat loss. Such a dual effect leads to the maximum temperature decreasing from 811.9 °C to 667.5 °C, and the maximum temperature rate declines up to 2.6 times. Correspondingly, the whole thermal runaway process is deferred, the total time increases from 370 s to 503 s, and the time interval, Δt, from safety venting gains by 32.3% as the ambient pressure and temperature decrease. This work delivers an in-depth understanding of the thermal characteristics under low pressure and low temperature and provides meritorious guidance for the safety of cell transportation in aviation. Full article

(This article belongs to the Section Battery Performance, Ageing, Reliability and Safety)

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12 pages, 4328 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

A Novel Reaction Rate Parametrization Method for Lithium-Ion Battery Electrochemical Modelling

by Alain Goussian, Loïc Assaud, Issam Baghdadi, Cédric Nouillant and Sylvain Franger

Batteries 2024, 10(6), 205; https://doi.org/10.3390/batteries10060205 - 14 Jun 2024

Cited by 3 | Viewed by 2331

Abstract

To meet the ever-growing worldwide electric vehicle demand, the development of advanced generations of lithium-ion batteries is required. To this end, modelling is one of the pillars for the innovation process. However, modelling batteries containing a large number of different mechanisms occurring at [...] Read more.

To meet the ever-growing worldwide electric vehicle demand, the development of advanced generations of lithium-ion batteries is required. To this end, modelling is one of the pillars for the innovation process. However, modelling batteries containing a large number of different mechanisms occurring at different scales remains a field of research that does not provide consensus for each particular model or approach. Parametrization as part of the modelling process appears to be one of the issues when it comes to building a high-fidelity model of a target cell. In this paper, a particular parameter identification is therefore discussed. Indeed, even if Butler–Volmer is a well-known equation in the electrochemistry field, identification of its reaction rate constant or exchange current density parameters is lacking in the literature. Thus, we discuss the process described in the literature and propose a new protocol that expects to overcome certain difficulties whereas the hypothesis of calculation and measurement maintains high sensitivity. Full article

(This article belongs to the Special Issue Modeling, Reliability and Health Management of Lithium-Ion Batteries)

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13 pages, 6231 KiB

Open AccessEditor’s ChoiceArticle

Quantitative Analysis of Lithium-Ion Battery Eruption Behavior in Thermal Runaway

by Yu Xing, Ningning Wei and Minghai Li

Batteries 2024, 10(6), 182; https://doi.org/10.3390/batteries10060182 - 26 May 2024

Viewed by 2256

Abstract

With the widespread adoption of battery technology in electric vehicles, there has been significant attention drawn to the increasing frequency of battery fire incidents. However, the jetting behavior and expansion force during the thermal runaway (TR) of batteries represent highly dynamic phenomena, which [...] Read more.

With the widespread adoption of battery technology in electric vehicles, there has been significant attention drawn to the increasing frequency of battery fire incidents. However, the jetting behavior and expansion force during the thermal runaway (TR) of batteries represent highly dynamic phenomena, which lack comprehensive quantitative description. This study addresses this gap by employing an enhanced experimental setup that synchronizes the video timing of cameras with a signal acquisition system, enabling the multidimensional quantification of signals, such as images, temperature, voltage, and pressure. It also provides a detailed description of the jetting behavior and expansion force characteristics over time for Li(Ni_0.8Co_0.1Mn_0.1)O₂ batteries undergoing thermal runaway in an open environment. The results from three experiments effectively identify key temporal features, including the timing of the initial jetting spark, maximum jetting velocity, jetting duration, explosion duration, and patterns of flame volume variation. This quantitative analytical approach proves effective across various battery types and conditions. The findings could offer scientific foundations and experimental strategies for parameter identification in fire prevention and thermal runaway model development. Full article

(This article belongs to the Special Issue Battery Thermal Performance and Management: Advances and Challenges)

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21 pages, 2358 KiB

Open AccessFeature PaperEditor’s ChoiceReview

Useful Quantities and Diagram Types for Diagnosis and Monitoring of Electrochemical Energy Converters Using Impedance Spectroscopy: State of the Art, Review and Outlook

by Peter Kurzweil, Wolfgang Scheuerpflug, Christian Schell and Josef Schottenbauer

Batteries 2024, 10(6), 177; https://doi.org/10.3390/batteries10060177 - 24 May 2024

Cited by 4 | Viewed by 1840

Abstract

The concept of pseudocapacitance is explored as a rapid and universal method for the state of health (SOH) determination of batteries and supercapacitors. In contrast to this, the state of the art considers the degradation of a series of full charge/discharge cycles. Lithium-ion [...] Read more.

The concept of pseudocapacitance is explored as a rapid and universal method for the state of health (SOH) determination of batteries and supercapacitors. In contrast to this, the state of the art considers the degradation of a series of full charge/discharge cycles. Lithium-ion batteries, sodium-ion batteries and supercapacitors of different cell chemistries are studied by impedance spectroscopy during lifetime testing. Faradaic and capacitive charge storage are distinguished by the relationship between the stored electric charge and capacitance. Batteries with a flat voltage–charge curve are best suited for impedance spectroscopy. There is a slight loss in the linear correlation between the pseudocapacitance and Ah capacity in regions of overcharge and deep discharge. The correct calculation of quantities related to complex impedance and differential capacitance is outlined, which may also be useful as an introductory text and tutorial for newcomers to the field. Novel diagram types are proposed for the purpose of the instant performance and failure diagnosis of batteries and supercapacitors. Full article

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51 pages, 24057 KiB

Open AccessEditor’s ChoiceArticle

Biomass-Derived Carbon Materials for Advanced Metal-Ion Hybrid Supercapacitors: A Step Towards More Sustainable Energy

by Syed Shaheen Shah

Batteries 2024, 10(5), 168; https://doi.org/10.3390/batteries10050168 - 20 May 2024

Cited by 23 | Viewed by 5581

Abstract

Modern research has made the search for high-performance, sustainable, and efficient energy storage technologies a main focus, especially in light of the growing environmental and energy-demanding issues. This review paper focuses on the pivotal role of biomass-derived carbon (BDC) materials in the development [...] Read more.

Modern research has made the search for high-performance, sustainable, and efficient energy storage technologies a main focus, especially in light of the growing environmental and energy-demanding issues. This review paper focuses on the pivotal role of biomass-derived carbon (BDC) materials in the development of high-performance metal-ion hybrid supercapacitors (MIHSCs), specifically targeting sodium (Na)-, potassium (K)-, aluminium (Al)-, and zinc (Zn)-ion-based systems. Due to their widespread availability, renewable nature, and exceptional physicochemical properties, BDC materials are ideal for supercapacitor electrodes, which perfectly balance environmental sustainability and technological advancement. This paper delves into the synthesis, functionalization, and structural engineering of advanced biomass-based carbon materials, highlighting the strategies to enhance their electrochemical performance. It elaborates on the unique characteristics of these carbons, such as high specific surface area, tuneable porosity, and heteroatom doping, which are pivotal in achieving superior capacitance, energy density, and cycling stability in Na-, K-, Al-, and Zn-ion hybrid supercapacitors. Furthermore, the compatibility of BDCs with metal-ion electrolytes and their role in facilitating ion transport and charge storage mechanisms are critically analysed. Novelty arises from a comprehensive comparison of these carbon materials across metal-ion systems, unveiling the synergistic effects of BDCs’ structural attributes on the performance of each supercapacitor type. This review also casts light on the current challenges, such as scalability, cost-effectiveness, and performance consistency, offering insightful perspectives for future research. This review underscores the transformative potential of BDC materials in MIHSCs and paves the way for next-generation energy storage technologies that are both high-performing and ecologically friendly. It calls for continued innovation and interdisciplinary collaboration to explore these sustainable materials, thereby contributing to advancing green energy technologies. Full article

(This article belongs to the Special Issue Advanced Studies on High-Performance Metal-Ion Capacitors: Technologies, Systems and Applications)

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39 pages, 9443 KiB

Open AccessEditor’s ChoiceReview

Empowering Electric Vehicles Batteries: A Comprehensive Look at the Application and Challenges of Second-Life Batteries

by Seyedreza Azizighalehsari, Prasanth Venugopal, Deepak Pratap Singh, Thiago Batista Soeiro and Gert Rietveld

Batteries 2024, 10(5), 161; https://doi.org/10.3390/batteries10050161 - 14 May 2024

Cited by 12 | Viewed by 8143

Abstract

The surge in electric vehicle adoption has resulted in a significant rise in end-of-life batteries, which are unsuitable for demanding EV applications. Repurposing these batteries for secondary applications presents a promising avenue to tackle environmental and economic challenges associated with their disposal. The [...] Read more.

The surge in electric vehicle adoption has resulted in a significant rise in end-of-life batteries, which are unsuitable for demanding EV applications. Repurposing these batteries for secondary applications presents a promising avenue to tackle environmental and economic challenges associated with their disposal. The second-life battery (SLB) approach emerges as a mechanism to manage this massive amount of retired EV batteries. However, this approach poses significant challenges in determining and monitoring battery degradation and performance. After evaluating different scenarios for reusing or recycling retired EV batteries, this paper examines the main challenges associated with SLBs, including techno-economic aspects, uncertainty from first life, safety, characterization and screening, battery-management systems, and secondary applications. A comprehensive review of current state-of-the-art SLB research and implementations is provided, particularly emphasizing battery characterization and the requisite evaluation processes for SLB eligibility. This paper explores diverse measurement techniques for assessing SLB performance, evaluating them based on accuracy, complexity, and time consumption, which are essential for achieving cost-effective SLB applications. The overarching objective is to thoroughly understand the principal challenges associated with repurposing EV batteries and delineate the research imperatives necessary for their successful implementation and prolonged lifespan. Full article

(This article belongs to the Special Issue Recycling and Reuse of End-of-Life Lithium-Ion Batteries: Challenges and Strategies)

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26 pages, 2299 KiB

Open AccessEditor’s ChoiceReview

A Comparative Review of Models for All-Solid-State Li-Ion Batteries

by Erkin Yildiz, Mattia Serpelloni, Alberto Salvadori and Luigi Cabras

Batteries 2024, 10(5), 150; https://doi.org/10.3390/batteries10050150 - 29 Apr 2024

Cited by 5 | Viewed by 5047

Abstract

In recent times, there has been significant enthusiasm for the development of all-solid-state Li-ion batteries. This interest stems from a dual focus on safety—addressing concerns related to toxic and flammable organic liquid electrolytes—and the pursuit of high energy density. While liquid electrolyte batteries [...] Read more.

In recent times, there has been significant enthusiasm for the development of all-solid-state Li-ion batteries. This interest stems from a dual focus on safety—addressing concerns related to toxic and flammable organic liquid electrolytes—and the pursuit of high energy density. While liquid electrolyte batteries currently constitute the vast majority of commercial cells, solid electrolyte batteries show great promise. In parallel with experimental research, computational models clarify several fundamental physics that take place throughout battery operations. Giving up on reviewing a broad screening of the existing literature, we set out to select here a few highly relevant models, emphasizing some fundamental conceptual advancements and offering an in-depth and critical insight into the current state of the art. The papers we selected aim at providing the reader with a tangible and quantitative understanding of how all-solid-state Li-ion batteries operate, including the different mechanisms at play and the mathematical tools required to model the pertinent physics and mechanics. Full article

(This article belongs to the Section Battery Modelling, Simulation, Management and Application)

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20 pages, 2268 KiB

Open AccessEditor’s ChoiceArticle

Mechanical Measurement Approach to Characterize Venting Behavior during Thermal Runaway of 18650 Format Lithium-Ion Batteries

by Elisabeth Irene Gillich, Marco Steinhardt, Yaroslava Fedoryshyna and Andreas Jossen

Batteries 2024, 10(4), 142; https://doi.org/10.3390/batteries10040142 - 22 Apr 2024

Cited by 3 | Viewed by 3971

Abstract

The propagation of thermal runaway in a battery system is safety-critical in almost every application, such as electric vehicles or home storage. Abuse models can help to undestand propagation mechanisms and assist in designing safe battery systems, but need to be well-parametrized. Most [...] Read more.

The propagation of thermal runaway in a battery system is safety-critical in almost every application, such as electric vehicles or home storage. Abuse models can help to undestand propagation mechanisms and assist in designing safe battery systems, but need to be well-parametrized. Most of the heat during thermal runaway is released by venting that is why the characteristic of the vent flow plays an important part in the safety assessment. During venting, the cell generates a recoil force like a rocket, which depends on the flow speed and flow rate of the gas. This principle is used in this work to measure the velocity and mass flow rate of the vent gas. High-power and high-energy 18650 format lithium-ion batteries were overheated and the recoil and weight forces were measured to determine the venting parameter during thermal runaway. Our results show, that the linearized gas flow rate for the high-power and high-energy cell is

22.15 {gs}^{- 1}

and

27.92 {gs}^{- 1}

, respectively. The progress of the gas velocity differs between the two cell types and in case of the high-energy cell, it follows a single peak asymmetrical pattern with a peak of

398.5 {ms}^{- 1}

, while the high-power cell shows a bumpy pattern with a maximum gas velocity of

260.9 {ms}^{- 1}

. The developed test bench and gained results can contribute insights in the venting behavior, characterize venting, support safety assessments, simulations and pack design studies. Full article

(This article belongs to the Section Battery Performance, Ageing, Reliability and Safety)

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15 pages, 9500 KiB

Open AccessEditor’s ChoiceArticle

Postmortem Analysis of 18650 Graphite/LFP Cells in a Long-Term Aging Study for Second-Life Applications

by William Wheeler, Yann Bultel, Pascal Venet, Ali Sari and Elie Riviere

Batteries 2024, 10(4), 119; https://doi.org/10.3390/batteries10040119 - 2 Apr 2024

Cited by 3 | Viewed by 3670

Abstract

Second-life applications for lithium-ion batteries offer industry opportunities to defer recycling costs, enhance economic value, and reduce environmental impacts. However, cells are affected by numerous aging phenomena which can lead to an acceleration in capacity loss. This paper uses postmortem techniques to compare [...] Read more.

Second-life applications for lithium-ion batteries offer industry opportunities to defer recycling costs, enhance economic value, and reduce environmental impacts. However, cells are affected by numerous aging phenomena which can lead to an acceleration in capacity loss. This paper uses postmortem techniques to compare aging phenomenon in 1.1 Ah 18650 graphite/LFP cells, examining the differences between a pristine cell and three cells aged to 40~30% of state of health (SoH). Macroscopic and microscopic techniques are used to identify aging phenomenon occurring in the cell on both positive and negative electrodes. Energy-dispersive X-ray spectroscopy (EDXS) and scanning electron microscopes (SEMs) with back-scattered electron (BSE) detector are used to analyze each electrode. These methods are used to analyze the morphology and the material on each electrode. The results show a stable positive LFP electrode whereas numerous deposits and cracking occurred on the negative electrode. A discussion of the appearance of those aging phenomenon is presented. Impacts for industrial cells in second-life applications are finally discussed. Full article

(This article belongs to the Section Battery Materials and Interfaces: Anode, Cathode, Separators and Electrolytes or Others)

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15 pages, 4255 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Diphenylphosphoryl Azide as a Multifunctional Flame Retardant Electrolyte Additive for Lithium-Ion Batteries

by Zhirui Li, Longfei Han, Yongchun Kan, Can Liao and Yuan Hu

Batteries 2024, 10(4), 117; https://doi.org/10.3390/batteries10040117 - 30 Mar 2024

Cited by 1 | Viewed by 2472

Abstract

Graphite anode materials and carbonate electrolyte have been the top choices for commercial lithium-ion batteries (LIBS) for a long time. However, the uneven deposition and stripping of lithium cause irreversible damage to the graphite structure, and the low flash point and high flammability [...] Read more.

Graphite anode materials and carbonate electrolyte have been the top choices for commercial lithium-ion batteries (LIBS) for a long time. However, the uneven deposition and stripping of lithium cause irreversible damage to the graphite structure, and the low flash point and high flammability of the carbonate electrolyte pose a significant fire safety risk. Here, we proposed a multifunctional electrolyte additive diphenylphosphoryl azide (DPPA), which can construct a solid electrolyte interphase (SEI) with high ionic conductivity lithium nitride (Li₃N) to ensure efficient transport of Li⁺. This not only protects the artificial graphite (AG) electrode but also inhibits lithium dendrites to achieve excellent electrochemical performance. Meanwhile, the LIBS with DPPA offers satisfactory flame retardancy performance. The AG//Li half cells with DPPA-0.5M can still maintain a specific capacity of about 350 mAh/g after 200 cycles at 0.2 C. Its cycle performance and rate performance were better than commercial electrolyte (EC/DMC). After cycling, the microstructure surface of the AG electrode was complete and flat, and the surface of the lithium metal electrode had fewer lithium dendrites. Importantly, we found that the pouch cell with DPPA-0.5M had low peak heat release rate. When exposed to external conditions of continuous heating, DPPA significantly improved the fire safety of the LIBS. The research of DPPA in lithium electrolyte is a step towards the development of safe and efficient lithium batteries. Full article

(This article belongs to the Special Issue Advanced Materials and Technologies in All-Solid-State Lithium Batteries)

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14 pages, 12337 KiB

Open AccessEditor’s ChoiceArticle

Fast Impedance Spectrum Construction for Lithium-Ion Batteries Using a Multi-Density Clustering Algorithm

by Ling Zhu, Jichang Peng, Jinhao Meng, Chenghao Sun, Lei Cai and Zhizhu Qu

Batteries 2024, 10(3), 112; https://doi.org/10.3390/batteries10030112 - 20 Mar 2024

Cited by 3 | Viewed by 2710

Abstract

Effectively extracting a lithium-ion battery’s impedance is of great importance for various onboard applications, which requires consideration of both the time consumption and accuracy of the measurement process. Although the pseudorandom binary sequence (PRBS) excitation signal can inject the superposition frequencies with high [...] Read more.

Effectively extracting a lithium-ion battery’s impedance is of great importance for various onboard applications, which requires consideration of both the time consumption and accuracy of the measurement process. Although the pseudorandom binary sequence (PRBS) excitation signal can inject the superposition frequencies with high time efficiency and an easily implementable device, processing the data of the battery’s impedance measurement is still a challenge at present. This study proposes a fast impedance spectrum construction method for lithium-ion batteries, where a multi-density clustering algorithm was designed to effectively extract the useful impedance after PRBS injection. According to the distribution properties of the measurement points by PRBS, a density-based spatial clustering of applications with noise (DBSCAN) was used for processing the data of the lithium-ion battery’s impedance. The two key parameters of the DBSCAN were adjusted by a delicate workflow according to the frequency range. The validation of the proposed method was proved on a 3 Ah lithium-ion battery under nine different test conditions, considering both the SOC and temperature variations. Full article

(This article belongs to the Special Issue Artificial Intelligence-Based State-of-Health Estimation of Lithium-Ion Batteries—2nd Edition)

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29 pages, 2341 KiB

Open AccessFeature PaperEditor’s ChoiceReview

Safety Analysis of Lithium-Ion Cylindrical Batteries Using Design and Process Failure Mode and Effect Analysis

by Sahithi Maddipatla, Lingxi Kong and Michael Pecht

Batteries 2024, 10(3), 76; https://doi.org/10.3390/batteries10030076 - 23 Feb 2024

Cited by 12 | Viewed by 9555

Abstract

Cylindrical lithium-ion batteries are widely used in consumer electronics, electric vehicles, and energy storage applications. However, safety risks due to thermal runaway-induced fire and explosions have prompted the need for safety analysis methodologies. Though cylindrical batteries often incorporate safety devices, the safety of [...] Read more.

Cylindrical lithium-ion batteries are widely used in consumer electronics, electric vehicles, and energy storage applications. However, safety risks due to thermal runaway-induced fire and explosions have prompted the need for safety analysis methodologies. Though cylindrical batteries often incorporate safety devices, the safety of the battery also depends on its design and manufacturing processes. This study conducts a design and process failure mode and effect analysis (DFMEA and PFMEA) for the design and manufacturing of cylindrical lithium-ion batteries, with a focus on battery safety. Full article

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14 pages, 6593 KiB

Open AccessEditor’s ChoiceArticle

Influence of Pressure, Temperature and Discharge Rate on the Electrical Performances of a Commercial Pouch Li-Ion Battery

by Luigi Aiello, Peter Ruchti, Simon Vitzthum and Federico Coren

Batteries 2024, 10(3), 72; https://doi.org/10.3390/batteries10030072 - 21 Feb 2024

Cited by 11 | Viewed by 6781

Abstract

In this study, the performances of a pouch Li-ion battery (LIB) with respect to temperature, pressure and discharge-rate variation are measured. A sensitivity study has been conducted with three temperatures (5 °C, 25 °C, 45 °C), four pressures (0.2 MPa, 0.5 MPa, 0.8 [...] Read more.

In this study, the performances of a pouch Li-ion battery (LIB) with respect to temperature, pressure and discharge-rate variation are measured. A sensitivity study has been conducted with three temperatures (5 °C, 25 °C, 45 °C), four pressures (0.2 MPa, 0.5 MPa, 0.8 MPa, 1.2 MPa) and three electrical discharge rates (0.5 C, 1.5 C, 3.0 C). Electrochemical processes and overall efficiency are significantly affected by temperature and pressure, influencing capacity and charge–discharge rates. In previous studies, temperature and pressure were not controlled simultaneously due to technological limitations. A novel test bench was developed to investigate these influences by controlling the surface temperature and mechanical pressure on a pouch LIB during electrical charging and discharging. This test rig permits an accurate assessment of mechanical, thermal and electrical parameters, while decoupling thermal and mechanical influences during electrical operation. The results of the study confirm what has been found in the literature: an increase in pressure leads to a decrease in performance, while an increase in temperature leads to an increase in performance. However, the extent to which the pressure impacts performance is determined by the temperature and the applied electrical discharge rate. At 5 °C and 0.5 C, an increase in pressure from 0.2 MPa to 1.2 MPa results in a 5.84% decrease in discharged capacity. At 45 °C the discharge capacity decreases by 2.17%. Regarding the impact of the temperature, at discharge rate of 0.5 C, with an applied pressure of 0.2 MPa, an increase in temperature from 25 °C to 45 °C results in an increase of 4.27% in discharged capacity. The impact on performance varies significantly at different C-rates. Under the same pressure (0.2 MPa) and temperature variation (from 25 °C to 45 °C), increasing the electrical discharge rate to 1.5 C results in a 43.04% increase in discharged capacity. The interplay between temperature, pressure and C-rate has a significant, non-linear impact on performance. This suggests that the characterisation of an LIB would require the active control of both temperature and pressure during electrical operation. Full article

(This article belongs to the Special Issue Recent Advances in Battery Measurement and Management Systems)

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18 pages, 3439 KiB

Open AccessFeature PaperEditor’s ChoiceArticle

Heterogeneity of Lithium Distribution in the Graphite Anode of 21700-Type Cylindrical Li-Ion Cells during Degradation

by Dominik Petz, Volodymyr Baran, Juyeon Park, Alexander Schökel, Armin Kriele, Joana Rebelo Kornmeier, Carsten Paulmann, Max Koch, Tom Nilges, Peter Müller-Buschbaum and Anatoliy Senyshyn

Batteries 2024, 10(3), 68; https://doi.org/10.3390/batteries10030068 - 20 Feb 2024

Cited by 8 | Viewed by 4483

Abstract

Structural and spatial aspects of cell degradation are studied using a combination of diffraction-and imaging-based tools applying laboratory X-rays, neutron scattering and synchrotron radiation with electrochemical and thermal characterization. Experimental characterization is carried out on cylindrical cells of 21700-type, where four regimes of [...] Read more.

Structural and spatial aspects of cell degradation are studied using a combination of diffraction-and imaging-based tools applying laboratory X-rays, neutron scattering and synchrotron radiation with electrochemical and thermal characterization. Experimental characterization is carried out on cylindrical cells of 21700-type, where four regimes of cell degradation are identified, which are supplemented by an increased cell resistance and surface temperature during cell operation. The amount of intercalated lithium in the fully charged anodes in the fresh and aged states is determined by ex situ X-ray diffraction radiography and in situ X-ray diffraction computed tomography. The qualitatively similar character of the results revealed a loss of active lithium along with the development of a complex heterogeneous distribution over the electrode stripe. Full article

(This article belongs to the Section Battery Materials and Interfaces: Anode, Cathode, Separators and Electrolytes or Others)

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31 pages, 9263 KiB

Open AccessEditor’s ChoiceArticle

Bubble Wrap-like Carbon-Coated Rattle-Type silica@silicon Nanoparticles as Hybrid Anode Materials for Lithium-Ion Batteries via Surface-Protected Etching

by Angelica Martino, Jiyun Jeon, Hyun-Ho Park, Hochun Lee and Chang-Seop Lee

Batteries 2024, 10(2), 53; https://doi.org/10.3390/batteries10020053 - 1 Feb 2024

Cited by 2 | Viewed by 4236

Abstract

Severe volumetric expansion (~400%) limits practical application of silicon nanoparticles as anode materials for next-generation lithium-ion batteries (LIBs). Here, we describe the fabrication and characterization of a conformal polydopamine carbon shell encapsulating rattle-type silica@silicon nanoparticles (PDA–PEI@PVP–SiO₂@Si) with a tunable void structure [...] Read more.

Severe volumetric expansion (~400%) limits practical application of silicon nanoparticles as anode materials for next-generation lithium-ion batteries (LIBs). Here, we describe the fabrication and characterization of a conformal polydopamine carbon shell encapsulating rattle-type silica@silicon nanoparticles (PDA–PEI@PVP–SiO₂@Si) with a tunable void structure using a dual template strategy with TEOS and (3-aminopropyl)triethoxysilane (APTES) pretreated with polyvinylpyrrolidone (PVP K30) as SiO₂ sacrificial template via a modified Stöber process. Polyethylene imine (PEI) crosslinking facilitated the construction of an interconnected three-dimensional bubble wrap-like carbon matrix structure through hydrothermal treatment, pyrolysis, and subsequent surface-protected etching. The composite anode material delivered satisfactory capacities of 539 mAh g⁻¹ after 100 cycles at 0.1 A g⁻¹, 512.76 mAh g⁻¹ after 200 cycles at 1 A g⁻¹, and 453 mAh g⁻¹ rate performance at 5 A g⁻¹, respectively. The electrochemical performance of PDA–PEI@PVP–SiO₂@Si was attributed to the rattle-type structure providing void space for Si volume expansion, PVP K30-pretreated APTES/TEOS SiO₂ seeds via catalyst-free, hydrothermal-assisted Stöber protecting Si/C spheres upon etching, carbon coating strategy increasing Si conductivity while stabilizing the solid electrolyte interface (SEI), and PEI carbon crosslinks providing continuous conductive pathways across the electrode structure. The present work describes a promising strategy to synthesize tunable yolk shell C@void@Si composite anode materials for high power/energy-density LIBs applications. Full article

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20 pages, 15224 KiB

Open AccessEditor’s ChoiceArticle

Lithium-Ion Supercapacitors and Batteries for Off-Grid PV Applications: Lifetime and Sizing

by Tarek Ibrahim, Tamas Kerekes, Dezso Sera, Abderezak Lashab and Daniel-Ioan Stroe

Batteries 2024, 10(2), 42; https://doi.org/10.3390/batteries10020042 - 23 Jan 2024

Cited by 6 | Viewed by 3729

Abstract

The intermittent nature of power generation from photovoltaics (PV) requires reliable energy storage solutions. Using the storage system outdoors exposes it to variable temperatures, affecting both its storage capacity and lifespan. Utilizing and optimizing energy storage considering climatic variations and new storage technologies [...] Read more.

The intermittent nature of power generation from photovoltaics (PV) requires reliable energy storage solutions. Using the storage system outdoors exposes it to variable temperatures, affecting both its storage capacity and lifespan. Utilizing and optimizing energy storage considering climatic variations and new storage technologies is still a research gap. Therefore, this paper presents a modified sizing algorithm based on the Golden Section Search method, aimed at optimizing the number of cells in an energy storage unit, with a specific focus on the unique conditions of Denmark. The considered energy storage solutions are Lithium-ion capacitors (LiCs) and Lithium-ion batteries (LiBs), which are tested under different temperatures and C-rates rates. The algorithm aims to maximize the number of autonomy cycles—defined as periods during which the system operates independently of the grid, marked by intervals between two consecutive 0% State of Charge (SoC) occurrences. Testing scenarios include dynamic temperature and dynamic load, constant temperature at 25 °C, and constant load, considering irradiation and temperature effects and cell capacity fading over a decade. A comparative analysis reveals that, on average, the LiC storage is sized at 70–80% of the LiB storage across various scenarios. Notably, under a constant-temperature scenario, the degradation rate accelerates, particularly for LiBs. By leveraging the modified Golden Section Search algorithm, this study provides an efficient approach to the sizing problem, optimizing the number of cells and thus offering a potential solution for energy storage in off-grid PV systems. Full article

(This article belongs to the Special Issue Advances in Battery Status Estimation and Prediction)

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18 pages, 4251 KiB

Open AccessEditor’s ChoiceArticle

Spherical Graphite Anodes: Influence of Particle Size Distribution and Multilayer Structuring in Lithium-Ion Battery Cells

by Laura Gottschalk, Jannes Müller, Alexander Schoo, Ernesto Baasch and Arno Kwade

Batteries 2024, 10(2), 40; https://doi.org/10.3390/batteries10020040 - 23 Jan 2024

Cited by 8 | Viewed by 9284

Abstract

Current research focuses on lithium-ion battery cells with a high energy density and efficient fast-charging capabilities. However, transport limitations, and, therefore, the uniform diffusion of lithium-ions across the electrode layers, remain a challenge and could lead to reduced cell performance. One approach to [...] Read more.

Current research focuses on lithium-ion battery cells with a high energy density and efficient fast-charging capabilities. However, transport limitations, and, therefore, the uniform diffusion of lithium-ions across the electrode layers, remain a challenge and could lead to reduced cell performance. One approach to overcome these transport challenges is the use of subsequently produced two-layer anodes with the particle size variation of spherical graphite (x₅₀ = 18 µm; x₅₀ = 11 µm). Thereby, a defined pore network is created, which reduces the ionic resistance and ensuring improved fast charging capabilities. The analysis focuses on the evaluation of electrode properties and the electrochemical performance. By examining the pore size distribution of the anodes, it has been found that during the manufacturing of the two-layer anodes, carbon black and binder particles are transported into the existing microstructure of the lower layer, resulting in localized densification between the anode layers. This could also be supported by color measurements. This effect also extends to electrochemical investigations, with electrochemical impedance spectroscopy showing significantly lower ionic resistances in all two-layer anodes. Reduced ionic resistance and tortuosity near the separator due to absorption effects enhance the ion diffusion and have a direct impact on anode performance. Cell ageing analysis showed a significant capacity decrease of almost 15 mAh g ⁻¹ in the single-layer references only, in contrast to the stability of the two-layer anodes. This could also be attributed to the reduced ionic resistance and active counteraction of binder migration. In conclusion, this study highlights how subsequently produced two-layer anodes significantly shape the electrode properties and cell performance of lithium-ion batteries. Full article

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47 pages, 11199 KiB

Open AccessEditor’s ChoiceReview

Engineering Dry Electrode Manufacturing for Sustainable Lithium-Ion Batteries

by Mohamed Djihad Bouguern, Anil Kumar Madikere Raghunatha Reddy, Xia Li, Sixu Deng, Harriet Laryea and Karim Zaghib

Batteries 2024, 10(1), 39; https://doi.org/10.3390/batteries10010039 - 22 Jan 2024

Cited by 31 | Viewed by 26736

Abstract

The pursuit of industrializing lithium-ion batteries (LIBs) with exceptional energy density and top-tier safety features presents a substantial growth opportunity. The demand for energy storage is steadily rising, driven primarily by the growth in electric vehicles and the need for stationary energy storage [...] Read more.

The pursuit of industrializing lithium-ion batteries (LIBs) with exceptional energy density and top-tier safety features presents a substantial growth opportunity. The demand for energy storage is steadily rising, driven primarily by the growth in electric vehicles and the need for stationary energy storage systems. However, the manufacturing process of LIBs, which is crucial for these applications, still faces significant challenges in terms of both financial and environmental impacts. Our review paper comprehensively examines the dry battery electrode technology used in LIBs, which implies the use of no solvents to produce dry electrodes or coatings. In contrast, the conventional wet electrode technique includes processes for solvent recovery/drying and the mixing of solvents like N-methyl pyrrolidine (NMP). Methods that use dry films bypass the need for solvent blending and solvent evaporation processes. The advantages of dry processes include a shorter production time, reduced energy consumption, and lower equipment investment. This is because no solvent mixing or drying is required, making the production process much faster and, thus, decreasing the price. This review explores three solvent-free dry film techniques, such as extrusion, binder fibrillation, and dry spraying deposition, applied to LIB electrode coatings. Emphasizing cost-effective large-scale production, the critical methods identified are hot melting, extrusion, and binder fibrillation. This review provides a comprehensive examination of the solvent-free dry-film-making methods, detailing the underlying principles, procedures, and relevant parameters. Full article

(This article belongs to the Section Battery Materials and Interfaces: Anode, Cathode, Separators and Electrolytes or Others)

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30 pages, 6366 KiB

Open AccessEditor’s ChoiceReview

A Review of Lithium-Ion Battery Recycling: Technologies, Sustainability, and Open Issues

by Alessandra Zanoletti, Eleonora Carena, Chiara Ferrara and Elza Bontempi

Batteries 2024, 10(1), 38; https://doi.org/10.3390/batteries10010038 - 22 Jan 2024

Cited by 88 | Viewed by 40890

Abstract

Lithium-ion batteries (LIBs) are a widely used energy storage technology as they possess high energy density and are characterized by the reversible intercalation/deintercalation of Li ions between electrodes. The rapid development of LIBs has led to increased production efficiency and lower costs for [...] Read more.

Lithium-ion batteries (LIBs) are a widely used energy storage technology as they possess high energy density and are characterized by the reversible intercalation/deintercalation of Li ions between electrodes. The rapid development of LIBs has led to increased production efficiency and lower costs for manufacturers, resulting in a growing demand for batteries and their application across various industries, particularly in different types of vehicles. In order to meet the demand for LIBs while minimizing climate-impacting emissions, the reuse, recycling, and repurposing of LIBs is a critical step toward achieving a sustainable battery economy. This paper provides a comprehensive review of lithium-ion battery recycling, covering topics such as current recycling technologies, technological advancements, policy gaps, design strategies, funding for pilot projects, and a comprehensive strategy for battery recycling. Additionally, this paper emphasizes the challenges associated with developing LIB recycling and the opportunities arising from these challenges, such as the potential for innovation and the creation of a more sustainable and circular economy. The environmental implications of LIB recycling are also evaluated with methodologies able to provide a sustainability analysis of the selected technology. This paper aims to enhance the comprehension of these trade-offs and encourage discussion on determining the “best” recycling route when targets are in conflict. Full article

(This article belongs to the Special Issue Recycling and Reuse of End-of-Life Lithium-Ion Batteries: Challenges and Strategies)

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37 pages, 2206 KiB

Open AccessEditor’s ChoiceReview

Review on Modeling and SOC/SOH Estimation of Batteries for Automotive Applications

by Pierpaolo Dini, Antonio Colicelli and Sergio Saponara

Batteries 2024, 10(1), 34; https://doi.org/10.3390/batteries10010034 - 18 Jan 2024

Cited by 59 | Viewed by 15884

Abstract

Lithium-ion batteries have revolutionized the portable and stationary energy industry and are finding widespread application in sectors such as automotive, consumer electronics, renewable energy, and many others. However, their efficiency and longevity are closely tied to accurately measuring their SOC and state of [...] Read more.

Lithium-ion batteries have revolutionized the portable and stationary energy industry and are finding widespread application in sectors such as automotive, consumer electronics, renewable energy, and many others. However, their efficiency and longevity are closely tied to accurately measuring their SOC and state of health (SOH). The need for precise algorithms to estimate SOC and SOH has become increasingly critical in light of the widespread adoption of lithium-ion batteries in industrial and automotive applications. While the benefits of lithium-ion batteries are undeniable, the challenges related to their efficient and safe management cannot be overlooked. Accurate estimation of SOC and SOH is crucial for ensuring optimal battery management, maximizing battery lifespan, optimizing performance, and preventing sudden failures. Consequently, research and development of reliable algorithms for estimating SOC and SOH have become an area of growing interest for the scientific and industrial community. This review article aims to provide an in-depth analysis of the state-of-the-art in SOC and SOH estimation algorithms for lithium-ion batteries. The most recent and promising theoretical and practical techniques used to address the challenges of accurate SOC and SOH estimation will be examined and evaluated. Additionally, critical evaluation of different approaches will be highlighted: emphasizing the advantages, limitations, and potential areas for improvement. The goal is to provide a clear view of the current landscape and to identify possible future directions for research and development in this crucial field for technological innovation. Full article

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36 pages, 5743 KiB

Open AccessEditor’s ChoiceReview

Advancements and Challenges in Solid-State Battery Technology: An In-Depth Review of Solid Electrolytes and Anode Innovations

by Abniel Machín, Carmen Morant and Francisco Márquez

Batteries 2024, 10(1), 29; https://doi.org/10.3390/batteries10010029 - 17 Jan 2024

Cited by 67 | Viewed by 39972

Abstract

The primary goal of this review is to provide a comprehensive overview of the state-of-the-art in solid-state batteries (SSBs), with a focus on recent advancements in solid electrolytes and anodes. The paper begins with a background on the evolution from liquid electrolyte lithium-ion [...] Read more.

The primary goal of this review is to provide a comprehensive overview of the state-of-the-art in solid-state batteries (SSBs), with a focus on recent advancements in solid electrolytes and anodes. The paper begins with a background on the evolution from liquid electrolyte lithium-ion batteries to advanced SSBs, highlighting their enhanced safety and energy density. It addresses the increasing demand for efficient, safe energy storage in applications like electric vehicles and portable electronics. A major part of the paper analyzes solid electrolytes, key to SSB technology. It classifies solid electrolytes as polymer-based, oxide-based, and sulfide-based, discussing their distinct properties and application suitability. The review also covers advancements in anode materials for SSBs, exploring materials like lithium metal, silicon, and intermetallic compounds, focusing on their capacity, durability, and compatibility with solid electrolytes. It addresses challenges in integrating these anode materials, like the interface stability and lithium dendrite growth. This review includes a discussion on the latest analytical techniques, experimental studies, and computational models to understand and improve the anode–solid electrolyte interface. These are crucial for tackling interfacial resistance and ensuring SSBs’ long-term stability and efficiency. Concluding, the paper suggests future research and development directions, highlighting SSBs’ potential in revolutionizing energy storage technologies. This review serves as a vital resource for academics, researchers, and industry professionals in advanced battery technology development. It offers a detailed overview of materials and technologies shaping SSBs’ future, providing insights into current challenges and potential solutions in this rapidly evolving field. Full article

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18 pages, 8368 KiB

Open AccessEditor’s ChoiceArticle

Design and Control of a Modular Integrated On-Board Battery Charger for EV Applications with Cell Balancing

by Fatemeh Nasr Esfahani, Ahmed Darwish and Xiandong Ma

Batteries 2024, 10(1), 17; https://doi.org/10.3390/batteries10010017 - 2 Jan 2024

Cited by 9 | Viewed by 4134

Abstract

This paper presents operation and control systems for a new modular on-board charger (OBC) based on a SEPIC converter (MSOBC) for electric vehicle (EV) applications. The MSOBC aims to modularise the battery units in the energy storage system of the EV to provide [...] Read more.

This paper presents operation and control systems for a new modular on-board charger (OBC) based on a SEPIC converter (MSOBC) for electric vehicle (EV) applications. The MSOBC aims to modularise the battery units in the energy storage system of the EV to provide better safety and improved operation. This is mainly achieved by reducing the voltage of the battery packs without sacrificing the performance required by the HV system. The proposed MSOBC is an integrated OBC which can operate the EV during traction and braking, as well as charge the battery units. The MSOBC is composed of several submodules consisting of a full-bridge voltage source converter connected on the ac side and SEPIC converter installed on the battery side. The SEPIC converter controls the battery segments with a continuous current because it has an input inductor which can smooth the battery’s currents without the need for large electrolytic capacitors. The isolated version of the SEPIC converter is employed to enhance the system’s safety by providing galvanic isolation between the batteries and the ac output side. This paper presents the necessary control loops to ensure the optimal operation of the EV with the MSOBC in terms of charge and temperature balance without disturbing the required modes of operation. The mathematical analyses in this paper are validated using a full-scale EV controlled by TMS320F28335 DSP. Full article

(This article belongs to the Special Issue Advances in Battery Electric Vehicles)

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12 pages, 2695 KiB

Open AccessEditor’s ChoiceArticle

Percolation Behavior of a Sulfide Electrolyte–Carbon Additive Matrix for Composite Cathodes in All-Solid-State Batteries

by Elias Reisacher, Pinar Kaya and Volker Knoblauch

Batteries 2023, 9(12), 595; https://doi.org/10.3390/batteries9120595 - 15 Dec 2023

Cited by 3 | Viewed by 3529

Abstract

To achieve high energy densities with sufficient cycling performance in all-solid-state batteries, the fraction of active material has to be maximized while maintaining ionic and electronic conduction throughout the composite cathode. It is well known that low-surface-area carbon additives added to the composite [...] Read more.

To achieve high energy densities with sufficient cycling performance in all-solid-state batteries, the fraction of active material has to be maximized while maintaining ionic and electronic conduction throughout the composite cathode. It is well known that low-surface-area carbon additives added to the composite cathode enhance the rate capability; however, at the same time, they can lead to rapid decomposition of the solid electrolyte in thiophosphate-based cells. Thus, the fraction of such conductive additives has to be well balanced. Within this study we determined the electronic percolation threshold of a conducting matrix consisting of Li₆PS₅Cl and C65. Furthermore, we systematically investigated the microstructure and effective conductivity (σ_eff) of the conducting matrix. The percolation threshold p_c was determined as ~4 wt.-% C65, and it is suggested that below p_c, the ionic contribution is dominant, which can be seen in temperature-dependent σ_eff and blocked charge transport at low frequencies. Above p_c, the impedance of the conducting matrix becomes frequency-independent, and the ohmic law applies. Thus, the conducting matrix in ASSB can be regarded as an electronic and ionic conducting phase between active material particles. Additionally, guidelines are provided to enable electronic conduction in the conducting matrix with minimal C65 content. Full article

(This article belongs to the Topic Advances in Energy Storage Materials/Devices and Solid-State Batteries)

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16 pages, 2918 KiB

Open AccessEditor’s ChoiceArticle

Qualitative Characterization of Lead–Acid Batteries Fabricated Using Different Technological Procedures: An EIS Approach

by Olivia Bruj and Adrian Calborean

Batteries 2023, 9(12), 593; https://doi.org/10.3390/batteries9120593 - 14 Dec 2023

Viewed by 3292

Abstract

Electrochemical impedance spectroscopy techniques were applied in this work to nine industrially fabricated lead–acid battery prototypes, which were divided into three type/technology packages. Frequency-dependent impedance changes were interpreted during successive charge/discharge cycles in two distinct stages: (1) immediately after fabrication and (2) after [...] Read more.

Electrochemical impedance spectroscopy techniques were applied in this work to nine industrially fabricated lead–acid battery prototypes, which were divided into three type/technology packages. Frequency-dependent impedance changes were interpreted during successive charge/discharge cycles in two distinct stages: (1) immediately after fabrication and (2) after a controlled aging procedure to 50% depth of discharge following industrial standards. To investigate their state of health behavior vs. electrical response, three methods were employed, namely, the Q-Q₀ total charge analysis, the decay values of the constant-phase element in the equivalent Randles circuits, and the resonance frequency of the circuit. A direct correlation was found for the prediction of the best-performing batteries in each package, thus allowing for a qualitative analysis that was capable of providing the decay of the batteries’ states of health. We found which parameters were directly connected with their lifetime performance in both stages and, as a consequence, which type/technology battery prototype displayed the best performance. Based on this methodology, industrial producers can further establish the quality of novel batteries in terms of performance vs. lifespan, allowing them to validate the novel technological innovations implemented in the current prototypes. Full article

(This article belongs to the Special Issue Electrochemistry of Lead-Acid Batteries)

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10 pages, 1035 KiB

Open AccessEditor’s ChoiceArticle

Silicon Negative Electrodes—What Can Be Achieved for Commercial Cell Energy Densities

by William Yourey

Batteries 2023, 9(12), 576; https://doi.org/10.3390/batteries9120576 - 28 Nov 2023

Cited by 1 | Viewed by 2649

Abstract

Historically, lithium cobalt oxide and graphite have been the positive and negative electrode active materials of choice for commercial lithium-ion cells. It has only been over the past ~15 years in which alternate positive electrode materials have been used. As new positive and [...] Read more.

Historically, lithium cobalt oxide and graphite have been the positive and negative electrode active materials of choice for commercial lithium-ion cells. It has only been over the past ~15 years in which alternate positive electrode materials have been used. As new positive and negative active materials, such as NMC811 and silicon-based electrodes, are being developed, it is crucial to evaluate the potential of these materials at a stack or cell level to fully understand the possible increases in energy density which can be achieved. Comparisons were made between electrode stack volumetric energy densities for designs containing either LCO or NMC811 positive electrode and silicon-graphite negative electrodes, where the weight percentages of silicon were evaluated between zero and ninety percent. Positive electrode areal loadings were evaluated between 2.00 and 5.00 mAh cm⁻². NMC811 at 200 mAh g⁻¹ has the ability to increase stack energy density between 11% and 20% over LCO depending on percentage silicon and areal loading. At a stack level, the percentage of silicon added results in large increases in energy density but delivers a diminishing return, with the greatest increase observed as the percentage of silicon is increased from zero percent to approximately 25–30%. Full article

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22 pages, 4151 KiB

Open AccessEditor’s ChoiceReview

Second-Life Batteries: A Review on Power Grid Applications, Degradation Mechanisms, and Power Electronics Interface Architectures

by Ali Hassan, Shahid Aziz Khan, Rongheng Li, Wencong Su, Xuan Zhou, Mengqi Wang and Bin Wang

Batteries 2023, 9(12), 571; https://doi.org/10.3390/batteries9120571 - 27 Nov 2023

Cited by 18 | Viewed by 9573

Abstract

The adoption of electric vehicles (EVs) is increasing due to governmental policies focused on curbing climate change. EV batteries are retired when they are no longer suitable for energy-intensive EV operations. A large number of EV batteries are expected to be retired in [...] Read more.

The adoption of electric vehicles (EVs) is increasing due to governmental policies focused on curbing climate change. EV batteries are retired when they are no longer suitable for energy-intensive EV operations. A large number of EV batteries are expected to be retired in the next 5–10 years. These retired batteries have 70–80% average capacity left. Second-life use of these battery packs has the potential to address the increasing energy storage system (ESS) demand for the grid and also to create a circular economy for EV batteries. The needs of modern grids for frequency regulation, power smoothing, and peak shaving can be met using retired batteries. Moreover, these batteries can also be employed for revenue generation for energy arbitrage (EA). While there are articles reviewing the general applications of retired batteries, this paper presents a comprehensive review of the research work on applications of the second-life batteries (SLBs) specific to the power grid and SLB degradation. The power electronics interface and battery management systems for the SLB are also thoroughly reviewed. Full article

(This article belongs to the Special Issue Second-Life Batteries)

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16 pages, 3567 KiB

Open AccessEditor’s ChoiceArticle

Sustainable Lithium Ferro-Phosphate Cathode Manufacturing: A Semi-Dry Approach with Water-Based Processing and Polytetrafluorethylene Binders

by Eike Wiegmann, Steffen Fischer, Matthias Leeb and Arno Kwade

Batteries 2023, 9(12), 567; https://doi.org/10.3390/batteries9120567 - 24 Nov 2023

Cited by 7 | Viewed by 5114

Abstract

A novel water-based lithium ferro-phosphate (LFP) cathode manufacturing process characterized by a significant reduction in the amount of solvent has been developed (semi-dry). To establish and validate this new process, Polytetrafluorethylene (PTFE) is used as a binder, with a binder content of 1 [...] Read more.

A novel water-based lithium ferro-phosphate (LFP) cathode manufacturing process characterized by a significant reduction in the amount of solvent has been developed (semi-dry). To establish and validate this new process, Polytetrafluorethylene (PTFE) is used as a binder, with a binder content of 1 wt.%, minimizing the amount of inactive material within the electrode. Extrusion screws with multiple kneading zones stress the PTFE more intensively and thus produce more and smaller fibrils. The resulting extent of fibrillation is quantified by melting enthalpy as well as mechanical electrode properties. The degree of fibrillation of the binder in an electrode is known to influence the conductive electric and ionic pathways, which in turn affect the discharge capacity. It is shown that this process provides a flexible cathode layer that achieves a specific capacitance of 155 mAh g⁻¹ in initial cycling tests at 0.1 C. Compared to a conventionally processed LFP cathode, the discharge capacity and overall energy output are significantly increased, and the overall energy consumption decreases for the semi-dry processed LFP cathodes. Full article

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29 pages, 3715 KiB

Open AccessEditor’s ChoiceReview

Lithium-Ion Battery Manufacturing: Industrial View on Processing Challenges, Possible Solutions and Recent Advances

by Aslihan Örüm Aydin, Franziska Zajonz, Till Günther, Kamil Burak Dermenci, Maitane Berecibar and Lisset Urrutia

Batteries 2023, 9(11), 555; https://doi.org/10.3390/batteries9110555 - 15 Nov 2023

Cited by 28 | Viewed by 34576

Abstract

Developments in different battery chemistries and cell formats play a vital role in the final performance of the batteries found in the market. However, battery manufacturing process steps and their product quality are also important parameters affecting the final products’ operational lifetime and [...] Read more.

Developments in different battery chemistries and cell formats play a vital role in the final performance of the batteries found in the market. However, battery manufacturing process steps and their product quality are also important parameters affecting the final products’ operational lifetime and durability. In this review paper, we have provided an in-depth understanding of lithium-ion battery manufacturing in a chemistry-neutral approach starting with a brief overview of existing Li-ion battery manufacturing processes and developing a critical opinion of future prospectives, including key aspects such as digitalization, upcoming manufacturing technologies and their scale-up potential. In this sense, the review paper will promote an understanding of the process parameters and product quality. Full article

(This article belongs to the Section Battery Processing, Manufacturing and Recycling)

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13 pages, 4091 KiB

Open AccessEditor’s ChoiceArticle

Gaining a New Technological Readiness Level for Laser-Structured Electrodes in High-Capacity Lithium-Ion Pouch Cells

by Alexandra Meyer, Penghui Zhu, Anna Smith and Wilhelm Pfleging

Batteries 2023, 9(11), 548; https://doi.org/10.3390/batteries9110548 - 9 Nov 2023

Cited by 6 | Viewed by 3040

Abstract

For the first time, the laser structuring of large-footprint electrodes with a loading of 4 mAh cm⁻² has been validated in a relevant environment, including subsequent multi-layer stack cell assembly and electrochemical characterization of the resulting high-capacity lithium-ion pouch cell prototypes, i.e., [...] Read more.

For the first time, the laser structuring of large-footprint electrodes with a loading of 4 mAh cm⁻² has been validated in a relevant environment, including subsequent multi-layer stack cell assembly and electrochemical characterization of the resulting high-capacity lithium-ion pouch cell prototypes, i.e., a technological readiness level of 6 has been achieved for the 3D battery concept. The structuring was performed using a high-power ultrashort-pulsed laser, resulting in well-defined line structures in electrodes without damaging the current collector, and without melting or altering the battery active materials. For cells containing structured electrodes, higher charge and discharge capacities were measured for C-rates >1C compared to reference cells based on unstructured electrodes. In addition, cells with structured electrodes showed a three-fold increase in cycle lifetime at a C-rate of 1C compared to those with reference electrodes. Full article

(This article belongs to the Section Battery Performance, Ageing, Reliability and Safety)

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21 pages, 30585 KiB

Open AccessEditor’s ChoiceArticle

Arcing in Li-Ion Batteries

by Theo Ledinski, Andrey W. Golubkov, Oskar Schweighofer and Simon Erker

Batteries 2023, 9(11), 540; https://doi.org/10.3390/batteries9110540 - 31 Oct 2023

Cited by 9 | Viewed by 6337

Abstract

Lithium-Ion battery cells and automotive battery systems are constantly improving as a result of the rising popularity of electric vehicles. With higher energy densities of the cells, the risks in case of failure rise as well. In the worst case, a fast exothermic [...] Read more.

Lithium-Ion battery cells and automotive battery systems are constantly improving as a result of the rising popularity of electric vehicles. With higher energy densities of the cells, the risks in case of failure rise as well. In the worst case, a fast exothermic reaction known as thermal runaway can occur. During thermal runaway, the cell can emit around 66% of its mass as gas and particles. An experimental setup was designed and showed that the gas-particle-vent of a cell going through thermal runaway can cause electric breakthroughs. These breakthroughs could start electric arcing in the battery system, which could lead to additional damages such as burning through the casing or igniting the vent gas, making the damage more severe and difficult to control. Uncontrollable battery fires must be prevented. The emitted gas was analyzed and the ejected particles were examined to discuss the potential causes of the breakthroughs. Full article

(This article belongs to the Section Battery Modelling, Simulation, Management and Application)

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10 pages, 1622 KiB

Open AccessEditor’s ChoiceArticle

Microwave-Assisted Recovery of Spent LiCoO₂ Battery from the Corresponding Black Mass

by Matteo Scaglia, Antonella Cornelio, Alessandra Zanoletti, Daniele La Corte, Giada Biava, Ivano Alessandri, Angelo Forestan, Catya Alba, Laura Eleonora Depero and Elza Bontempi

Batteries 2023, 9(11), 536; https://doi.org/10.3390/batteries9110536 - 28 Oct 2023

Cited by 9 | Viewed by 4035

Abstract

The literature indicates that utilizing pyrometallurgical methods for processing spent LiCoO₂ (LCO) batteries can lead to cobalt recovery in the forms of Co₃O₄, CoO, and Co, while lithium can be retrieved as Li₂O or Li₂ [...] Read more.

The literature indicates that utilizing pyrometallurgical methods for processing spent LiCoO₂ (LCO) batteries can lead to cobalt recovery in the forms of Co₃O₄, CoO, and Co, while lithium can be retrieved as Li₂O or Li₂CO₃. However, the technology’s high energy consumption has also been noted as a challenge in this recovery process. Recently, an innovative and sustainable approach using microwave (MW) radiation has been proposed as an alternative to traditional pyrometallurgical methods for treating used lithium-ion batteries (LiBs). This method aims to address the shortcomings of the conventional approach. In this study, the treatment of the black mass (BM) from spent LCO batteries is explored for the first time using MW–materials interaction under an air atmosphere. The research reveals that the process can trigger carbothermic reactions. However, MW makes the BM so reactive that it causes rapid heating of the sample in a few minutes, also posing a fire risk. This paper presents and discusses the benefits and potential hazards associated with this novel technology for the recovery of spent LCO batteries and gives information about real samples of BM. The work opens the possibility of using a microwave for raw material recovery in spent LIBs, allowing to obtain rapid and more efficient reactions. Full article

(This article belongs to the Section Battery Processing, Manufacturing and Recycling)

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47 pages, 14335 KiB

Open AccessEditor’s ChoiceReview

A Review of Sodium-Metal Chloride Batteries: Materials and Cell Design

by Salvatore Gianluca Leonardi, Mario Samperi, Leone Frusteri, Vincenzo Antonucci and Claudia D’Urso

Batteries 2023, 9(11), 524; https://doi.org/10.3390/batteries9110524 - 24 Oct 2023

Cited by 8 | Viewed by 9508

Abstract

The widespread electrification of various sectors is triggering a strong demand for new energy storage systems with low environmental impact and using abundant raw materials. Batteries employing elemental sodium could offer significant advantages, as the use of a naturally abundant element such as [...] Read more.

The widespread electrification of various sectors is triggering a strong demand for new energy storage systems with low environmental impact and using abundant raw materials. Batteries employing elemental sodium could offer significant advantages, as the use of a naturally abundant element such as sodium is strategic to satisfy the increasing demand. Currently, lithium-ion batteries represent the most popular energy storage technology, owing to their tunable performance for various applications. However, where large energy storage systems are required, the use of expensive lithium-ion batteries could result disadvantageous. On the other hand, high-temperature sodium batteries represent a promising technology due to their theoretical high specific energies, high energy efficiency, long life and safety. Therefore, driven by the current market demand and the awareness of the potential that still needs to be exploited, research interest in high-temperature sodium batteries has regained great attention. This review aims to highlight the most recent developments on this topic, focusing on actual and prospective active materials used in sodium-metal chloride batteries. In particular, alternative formulations to conventional nickel cathodes and advanced ceramic electrolytes are discussed, referring to the current research challenges centered on cost reduction, lowering of the operating temperature and performance improvement. Moreover, a comprehensive overview on commercial tubular cell design and prototypal planar design is presented, highlighting advantages and limitations based on the analysis of research papers, patents and technical documents. Full article

(This article belongs to the Special Issue Recent Progress in Energy Storage Materials and Devices)

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15 pages, 2710 KiB

Open AccessEditor’s ChoiceArticle

Scale-Up of Lithium Iron Phosphate Cathodes with High Active Materials Contents for Lithium Ion Cells

by Geanina Apachitei, Rob Heymer, Michael Lain, Daniela Dogaru, Marc Hidalgo, James Marco and Mark Copley

Batteries 2023, 9(10), 518; https://doi.org/10.3390/batteries9100518 - 21 Oct 2023

Cited by 5 | Viewed by 5393

Abstract

The size of a lithium iron phosphate (LFP) cathode mix was increased by a factor of thirty, and the capacity of the cells produced with it by a factor of three-hundred. As well as rate and cycling tests, the coatings were also characterised [...] Read more.

The size of a lithium iron phosphate (LFP) cathode mix was increased by a factor of thirty, and the capacity of the cells produced with it by a factor of three-hundred. As well as rate and cycling tests, the coatings were also characterised for adhesion and resistivity. The adhesion and total through-plane resistance were both dependent on the drying conditions during coating. The discharge capacities at high rates and the pulse resistances showed much less influence from the drying temperature. The mix formulation contained 97 wt% LFP, and was based on an earlier design of experiments (DoE) study, using relatively high active material contents. Overall, the mix exceeded the performance predicted by the modelling study. Full article

(This article belongs to the Section Battery Processing, Manufacturing and Recycling)

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27 pages, 4817 KiB

Open AccessEditor’s ChoiceReview

Unraveling the Correlation between Structure and Lithium Ionic Migration of Metal Halide Solid-State Electrolytes via Neutron Powder Diffraction

by Hao Zhang, Feilong Xu, Xingyu Chen and Wei Xia

Batteries 2023, 9(10), 510; https://doi.org/10.3390/batteries9100510 - 15 Oct 2023

Cited by 6 | Viewed by 4258

Abstract

Metal halide solid-state electrolytes (SSEs) (Li-M-X system, typically Li₃MX₆ and Li₂MX_4; M is metal or rare-earth element, X is halogen) exhibit significant potential in all solid-state batteries (ASSB) due to wide stability windows (0.36–6.71 V vs. Li/Li [...] Read more.

Metal halide solid-state electrolytes (SSEs) (Li-M-X system, typically Li₃MX₆ and Li₂MX_4; M is metal or rare-earth element, X is halogen) exhibit significant potential in all solid-state batteries (ASSB) due to wide stability windows (0.36–6.71 V vs. Li/Li⁺), excellent compatibility with cathodes, and a water-mediated facile synthesis route for large-scale fabrication. Understanding the dynamics of Li⁺ transportation and the influence of the host lattice is the prerequisite for developing advanced Metal halide SSEs. Neutron powder diffraction (NPD), as the most cutting-edge technology, could essentially reflect the nuclear density map to determine the whole crystal structure. Through NPD, the Li+ distribution and occupation are clearly revealed for transport pathway analysis, and the influence of the host ion lattice on Li+ migration could be discussed. In this review, we stress NPD utilization in metal halide SSEs systems in terms of defect chemistry, phase transition, cation/anion disorder effects, dual halogen, lattice dynamics/polarizability, and in situ analysis of phase evolution. The irreplaceable role of NPD technology in designing metal halide SSEs with enhanced properties is stressed, and a perspective on future developments of NPD in metal halide SSEs is also presented. Full article

(This article belongs to the Special Issue Advanced Characterizations in Solid-State Batteries)

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14 pages, 5292 KiB

Open AccessEditor’s ChoiceArticle

A Layered Hybrid Oxide–Sulfide All-Solid-State Battery with Lithium Metal Anode

by Juliane Hüttl, Nicolas Zapp, Saoto Tanikawa, Kristian Nikolowski, Alexander Michaelis and Henry Auer

Batteries 2023, 9(10), 507; https://doi.org/10.3390/batteries9100507 - 10 Oct 2023

Cited by 4 | Viewed by 3628

Abstract

Different classes of solid electrolytes for all-solid-state batteries (ASSB) are currently being investigated, with each of them suitable for a different ASSB concept. Their combination in hybrid battery cells enables the use of their individual benefits while mitigating their disadvantages. The cubic stuffed [...] Read more.

Different classes of solid electrolytes for all-solid-state batteries (ASSB) are currently being investigated, with each of them suitable for a different ASSB concept. Their combination in hybrid battery cells enables the use of their individual benefits while mitigating their disadvantages. The cubic stuffed garnet Li₇La₃Zr₂O₁₂ (LLZO), for example, is stable in contact with metallic lithium but has only moderate ionic conductivity, whereas the thiophosphate Li₁₀SnP₂S₁₂ (LSPS) is processable using conventional battery manufacturing technologies and has an excellent lithium-ion conductivity but an inferior electrochemical stability. In this work, we, therefore, present a layered hybrid all-solid-state full-cell concept that accommodates a lithium metal anode, a LiNi_0.8Co_0.1Mn_0.1O₂-based composite cathode with an LSPS catholyte (LSPS/NCM811) and a sintered monolithic LLZO separator. The electrochemical stability of LLZO and LSPS at cathodic potentials (up to 4.2 V) was investigated via cyclic voltammetry in test cells, as well as by cycling half cells with LSPS or a mixed LSPS/LLZO catholyte. Furthermore, the pressure-dependency of the galvanostatic cycling of a Li | LLZO | LSPS/NCM811 full cell was investigated, as well as the according effect of the Li | LLZO interface in symmetric test cells. An operation pressure of 12.5 MPa was identified as the optimal value, which assures both sufficient inter-layer contact and impeded lithium penetration through the separator and cell short-circuiting. Full article

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18 pages, 5041 KiB

Open AccessEditor’s ChoiceReview

Molecular Engineering of Redox Couples for Non-Aqueous Redox Flow Batteries

by Casey M. Davis, Claire E. Boronski, Tianyi Yang, Tuo Liu and Zhiming Liang

Batteries 2023, 9(10), 504; https://doi.org/10.3390/batteries9100504 - 4 Oct 2023

Cited by 9 | Viewed by 4145

Abstract

Redox flow batteries (RFBs) have attracted significant attention as a promising electrochemical energy storage technology, offering various advantages such as grid-scale electricity production with variable intermittent electricity delivery, enhanced safety compared to metal-ion batteries, decoupled energy and power density, and simplified manufacturing processes. [...] Read more.

Redox flow batteries (RFBs) have attracted significant attention as a promising electrochemical energy storage technology, offering various advantages such as grid-scale electricity production with variable intermittent electricity delivery, enhanced safety compared to metal-ion batteries, decoupled energy and power density, and simplified manufacturing processes. For this review, we exclusively focus on organic, non-aqueous redox flow batteries. Specifically, we address the most recent progress and the major challenges related to the design and synthesis of robust redox-active organic compounds. An extensive examination of the synthesis and characterization of a wide spectrum of redox-active molecules, focusing particularly on derivatives of posolytes such as quinone, nitroxyl radicals, dialkoxybenzenes, and phenothiazine and negolytes such as viologen and pyridiniums, is provided. We explore the incorporation of various functional groups as documented in the references, aiming to enhance the chemical and electrochemical stability, as well as the solubility, of both the neutral and radical states of redox-active molecules. Additionally, we offer a comprehensive assessment of the cell-cycling performance exhibited by these redox-active molecules. Full article

(This article belongs to the Special Issue Energy Storage of Redox-Flow Batteries)

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12 pages, 2651 KiB

Open AccessEditor’s ChoiceArticle

Chemically and Physically Cross-Linked Inorganic–Polymer Hybrid Solvent-Free Electrolytes

by Yamato Kanai, Koji Hiraoka, Mutsuhiro Matsuyama and Shiro Seki

Batteries 2023, 9(10), 492; https://doi.org/10.3390/batteries9100492 - 26 Sep 2023

Viewed by 1997

Abstract

Safe, self-standing, all-solid-state batteries with improved solid electrolytes that have adequate mechanical strength, ionic conductivity, and electrochemical stability are strongly desired. Hybrid electrolytes comprising flexible polymers and highly conductive inorganic electrolytes must be compatible with soft thin films with high ionic conductivity. Herein, [...] Read more.

Safe, self-standing, all-solid-state batteries with improved solid electrolytes that have adequate mechanical strength, ionic conductivity, and electrochemical stability are strongly desired. Hybrid electrolytes comprising flexible polymers and highly conductive inorganic electrolytes must be compatible with soft thin films with high ionic conductivity. Herein, we propose a new type of solid electrolyte hybrid comprising a glass–ceramic inorganic electrolyte powder (Li_1+x+yAl_xTi_2−xSi_yP_3−yO₁₂; LICGC) in a poly(ethylene)oxide (PEO)-based polymer electrolyte that prevents decreases in ionic conductivity caused by grain boundary resistance. We investigated the cross-linking processes taking place in hybrid electrolytes. We also prepared chemically cross-linked PEO/LICGC and physically cross-linked poly(norbornene)/LICGC electrolytes, and evaluated them using thermal and electrochemical analyses, respectively. All of the obtained electrolyte systems were provided with homogenous, white, flexible, and self-standing thin films. The main ionic conductive phase changed from the polymer to the inorganic electrolyte at low temperatures (close to the glass transition temperature) as the LICGC concentration increased, and the Li⁺ ion transport number also improved. Cyclic voltammetry using [Li metal|Ni] cells revealed that Li was reversibly deposited/dissolved in the prepared hybrid electrolytes, which are expected to be used as new Li⁺-conductive solid electrolyte systems. Full article

(This article belongs to the Section Battery Materials and Interfaces: Anode, Cathode, Separators and Electrolytes or Others)

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20 pages, 1197 KiB

Open AccessEditor’s ChoiceArticle

Investigating the Production Atmosphere for Sulfide-Based Electrolyte Layers Regarding Occupational Health and Safety

by Tina Kreher, Patrick Jäger, Fabian Heim and Kai Peter Birke

Batteries 2023, 9(9), 472; https://doi.org/10.3390/batteries9090472 - 19 Sep 2023

Cited by 2 | Viewed by 3662

Abstract

In all-solid-state battery (ASSB) research, the importance of sulfide electrolytes is steadily increasing. However, several challenges arise concerning the future mass production of this class of electrolytes. Among others, the high reactivity with atmospheric moisture forming toxic and corrosive hydrogen sulfide (H₂ [...] Read more.

In all-solid-state battery (ASSB) research, the importance of sulfide electrolytes is steadily increasing. However, several challenges arise concerning the future mass production of this class of electrolytes. Among others, the high reactivity with atmospheric moisture forming toxic and corrosive hydrogen sulfide (H₂S) is a major issue. On a production scale, excessive exposure to H₂S leads to serious damage of production workers’ health, so additional occupational health and safety measures are required. This paper investigates the environmental conditions for the commercial fabrication of slurry-based sulfide solid electrolyte layers made of Li₃PS₄ (LPS) and Li₁₀GeP₂S₁₂ (LGPS) for ASSBs. First, the identification of sequential production steps and processing stages in electrolyte layer production is carried out. An experimental setup is used to determine the H₂S release of intermediates under different atmospheric conditions in the production chain, representative for the production steps. The H₂S release rates obtained on a laboratory scale are then scaled up to mass production dimensions and compared to occupational health and safety limits for protection against H₂S. It is shown that, under the assumptions made for the production of a slurry-based electrolyte layer with LPS or LGPS, a dry room with a dew point of

τ = - 40^{\circ} C

and an air exchange rate of

AER = 30 \frac{1}{h}

is sufficient to protect production workers from health hazards caused by H₂S. However, the synthesis of electrolytes requires an inert gas atmosphere, as the H₂S release rates are much higher compared to layer production. Full article

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20 pages, 7957 KiB

Open AccessEditor’s ChoiceReview

Understanding High-Voltage Behavior of Sodium-Ion Battery Cathode Materials Using Synchrotron X-ray and Neutron Techniques: A Review

by Vadim Shipitsyn, Rishivandhiga Jayakumar, Wenhua Zuo, Bing Sun and Lin Ma

Batteries 2023, 9(9), 461; https://doi.org/10.3390/batteries9090461 - 11 Sep 2023

Cited by 6 | Viewed by 4534

Abstract

Despite substantial research efforts in developing high-voltage sodium-ion batteries (SIBs) as high-energy-density alternatives to complement lithium-ion-based energy storage technologies, the lifetime of high-voltage SIBs is still associated with many fundamental scientific questions. In particular, the structure phase transition, oxygen loss, and cathode–electrolyte interphase [...] Read more.

Despite substantial research efforts in developing high-voltage sodium-ion batteries (SIBs) as high-energy-density alternatives to complement lithium-ion-based energy storage technologies, the lifetime of high-voltage SIBs is still associated with many fundamental scientific questions. In particular, the structure phase transition, oxygen loss, and cathode–electrolyte interphase (CEI) decay are intensely discussed in the field. Synchrotron X-ray and neutron scattering characterization techniques offer unique capabilities for investigating the complex structure and dynamics of high-voltage cathode behavior. In this review, to accelerate the development of stable high-voltage SIBs, we provide a comprehensive and thorough overview of the use of synchrotron X-ray and neutron scattering in studying SIB cathode materials with an emphasis on high-voltage layered transition metal oxide cathodes. We then discuss these characterizations in relation to polyanion-type cathodes, Prussian blue analogues, and organic cathode materials. Finally, future directions of these techniques in high-voltage SIB research are proposed, including CEI studies for polyanion-type cathodes and the extension of neutron scattering techniques, as well as the integration of morphology and phase characterizations. Full article

(This article belongs to the Special Issue Behavior of Cathode Materials at High Voltage)

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21 pages, 4912 KiB

Open AccessEditor’s ChoiceArticle

Model Development for Binder Migration within Lithium-Ion Battery Electrodes during the Drying Process

by Christiane Zihrul, Mark Lippke and Arno Kwade

Batteries 2023, 9(9), 455; https://doi.org/10.3390/batteries9090455 - 5 Sep 2023

Cited by 14 | Viewed by 5814

Abstract

In the drying process of electrodes for lithium-ion batteries, the layer structure is defined and can only be influenced slightly in the subsequent process steps. An essential point in the drying process is the fixation of the binder, ensuring both the adhesive and [...] Read more.

In the drying process of electrodes for lithium-ion batteries, the layer structure is defined and can only be influenced slightly in the subsequent process steps. An essential point in the drying process is the fixation of the binder, ensuring both the adhesive and cohesive strength of the electrode. It is known that high drying rates lead to the segregation of the binder in the direction of the coating surface, which results in reduced mechanical stability of the electrode. In a previous publication, an experimental approach was used to investigate the underlying processes that influence binder migration. These results are now used in a model-based approach to describe the binder migration using the convection–diffusion equation. The convective term originates from the shrinkage behavior of the layer during drying due to the relative movement between the active material particles and the solvent in which the binder is dissolved or dispersed; it is expected to be the cause of the binder migration. The diffusive term, representing the binder movement in the solvent, counteracts segregation. The interaction of these forces is simulated at different drying temperatures and the associated drying rates. Full article

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15 pages, 6975 KiB

Open AccessEditor’s ChoiceArticle

Thermal Propagation Test Bench with Multi Pouch Cell Setup for Reproducibility Investigations

by Björn Mulder, Jan Schöberl and Kai Peter Birke

Batteries 2023, 9(9), 447; https://doi.org/10.3390/batteries9090447 - 31 Aug 2023

Cited by 3 | Viewed by 2694

Abstract

Thermal propagation events of the traction batteries in electric vehicles are rare. However, their impact on the passengers in form of fire, smoke and heat can be severe. Current data on the dependencies and the reproducibility of thermal propagation is limited despite these [...] Read more.

Thermal propagation events of the traction batteries in electric vehicles are rare. However, their impact on the passengers in form of fire, smoke and heat can be severe. Current data on the dependencies and the reproducibility of thermal propagation is limited despite these major implications. Therefore, a thermal propagation test bench was developed for custom multi pouch experiments. This setup includes a multitude of temperature sensors throughout the module, voltage monitoring and a mass flow sensor. Two distinct experiments were initiated by nail penetration. These show a high degree of reproducibility thus allowing for future experiments regarding the dependencies of initial module temperatures and State of Charge (SoC) variations. Full article

(This article belongs to the Special Issue The Precise Battery—towards Digital Twins for Advanced Batteries)

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37 pages, 3234 KiB

Open AccessEditor’s ChoiceReview

Multiscale Modelling Methodologies of Lithium-Ion Battery Aging: A Review of Most Recent Developments

by Mir A. Ali, Carlos M. Da Silva and Cristina H. Amon

Batteries 2023, 9(9), 434; https://doi.org/10.3390/batteries9090434 - 24 Aug 2023

Cited by 16 | Viewed by 9027

Abstract

Lithium-ion batteries (LIBs) are leading the energy storage market. Significant efforts are being made to widely adopt LIBs due to their inherent performance benefits and reduced environmental impact for transportation electrification. However, achieving this widespread adoption still requires overcoming critical technological constraints impacting [...] Read more.

Lithium-ion batteries (LIBs) are leading the energy storage market. Significant efforts are being made to widely adopt LIBs due to their inherent performance benefits and reduced environmental impact for transportation electrification. However, achieving this widespread adoption still requires overcoming critical technological constraints impacting battery aging and safety. Battery aging, an inevitable consequence of battery function, might lead to premature performance losses and exacerbated safety concerns if effective thermo-electrical battery management strategies are not implemented. Battery aging effects must be better understood and mitigated, leveraging the predictive power of aging modelling methods. This review paper presents a comprehensive overview of the most recent aging modelling methods. Furthermore, a multiscale approach is adopted, reviewing these methods at the particle, cell, and battery pack scales, along with corresponding opportunities for future research in LIB aging modelling across these scales. Battery testing strategies are also reviewed to illustrate how current numerical aging models are validated, thereby providing a holistic aging modelling strategy. Finally, this paper proposes a combined multiphysics- and data-based modelling framework to achieve accurate and computationally efficient LIB aging simulations. Full article

(This article belongs to the Special Issue Feature Papers to Celebrate the First Impact Factor of Batteries)

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